TiO 2 , [6][7][8] and others [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] have been prepared and reported to have structurebased antibacterial properties. However, most of the methods used for fabricating surface nanopatterns require special equipment [3,5,18] and expensive starting materials, [3][4][5] and are only applicable to certain substrates. [3][4][6][7][8]19,24] It would be desirable to have a simple and scalable method for creating biocidal nanostructures on commonly used substrates for practical applications. [9,20] There is also an urgent need for biocompatible nanostructured surface coating technology for biomedical applications. Layered double hydroxides (LDHs) or anionic clays are wellstudied biocompatible materials that have attracted our attention. LDH itself is made from common elements, and it exists in nature (hydrotalcite) and are nontoxic. [25] They have a gen-, where M 2+ = Mg, Zn, Cu, Ni or Co, M 3+ = Al, Fe or Cr, and X n− = intercalating anion. M 2+ to M 3+ ratio is between 1 and 5. [26] Herein, we report a method of growing vertically aligned Mg-Al-LDH on various substrates. The as-prepared vertically aligned LDH (V-LDH) array showed very weak antibacterial properties against E. coli. However, after further modification, it demonstrated greatly enhanced antibacterial properties against Gram negative bacteria, Gram positive bacteria and fungi. The relationships between the antimicrobial properties and the surface sharpness, surface potential and hydrophilicity were investigated. We found that hydrophilicity has the greatest influence to the antibacterial properties of V-LDH. The inherent antibacterial property, intercalation capability and facile synthesis of V-LDH provide the potential for broad applications of this new antimicrobial material.